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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 451 records · Page 25
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Understanding the Roles of the Electrode/Electrolyte Interface for Enabling Stable Li∥Sulfurized Polyacrylonitrile Batteries

Sulfurized polyacrylonitrile (SPAN) is a promising high-capacity cathode material. Here, we use spatially resolved X-ray absorption spectroscopy combined with X-ray fluorescence (XRF) microscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy to examine the structural transformation of SPAN and the critical role of a robust cathode–electrolyte interface (CEI) on the electrode. LiS x species forms during the cycling of SPAN. However, in carbonate-based electrolytes and ether-based electrolytes with LiNO 3 additives, these species are well protected by the CEI and do not dissolve into the electrolytes. In contrast, in an ether-based electrolyte without the LiNO 3 additive, LiS x species dissolve into the electrolyte, resulting in the shuttle effect and capacity loss. Examination of the Li anode by XRF and SEM reveals dense spherical Li morphology in ether-based electrolytes, but sulfur is present in the absence of the LiNO 3 additive. In contrast, porous dendritic Li is found in the carbonate electrolyte. These analyses established that an ether-based electrolyte with LiNO 3 is a superior choice that enables stable cycling of both electrodes. Based on these insights, we successfully demonstrate the stable cycling of high areal loading SPAN cathode (>6.5 mA h cm –2 ) with lean electrolyte amounts, showing promising Li∥SPAN cell performance under practical conditions.

25 ENERGY STORAGE↗
DOE OSTI2025

Scalable Solution-Processed Electrolyte Membranes with Optimized Microstructure for High-Performance Protonic Ceramic Electrochemical Cells

Proton-conducting electrochemical cells (PCECs) are promising for efficient hydrogen production, but achieving dense, uniform, thin electrolyte layers remains a key challenge, particularly for scalable fabrication. Here, we present a solution-processed deposition approach with a mechanistically optimized slurry for uniform electrolyte formation. By tailoring particle size distribution, solid loading, and solvent/additive balance, we regulated wetting behavior and evaporation kinetics of the electrolyte slurry to promote homogeneous electrolyte particle packing. These features facilitate tight grain boundary contact and early stage neck growth during sintering, eliminating residual porosity, and improving mechanical integrity. The resulting ∼15 μm thick electrolyte shows high density, strong electrode adhesion, and stable interfaces outperforming the previously reported spray-based fabricated electrolyte by about 31% at 600 °C in FC mode. Single cells deliver 0.962 W cm –2 at 600 °C in fuel cell mode and 1.31 A cm –2 at 1.3 V in electrolysis mode, maintaining robust performance over 100 h with negligible degradation (≤0.02% h –1 ) in each mode. Scale-up to 2.5 cm diameter substrates confirmed reproducible densification and geometric stability. This work demonstrates a cost-effective, scalable route where control over particle-fluid interactions and drying dynamics enables a superior electrolyte microstructure and high PCEC performance.

dense microstructure↗
DOE OSTI2017

Deliberately Designed Atomic-Level Silver-Containing Interface Results in Improved Rate Capability and Utilization of Silver Hollandite for Lithium-Ion Storage

α-MnO 2 -structured materials are generally classified as semiconductors, thus we present a strategy to increase electrochemical utilization through design of a conductive material interface. Surface treatment of silver hollandite (Ag x Mn 8 O 16 ) with Ag + (Ag 2 O) provides significant benefit to the resultant electrochemistry, including a decreased charge transfer resistance, and a 2-fold increase in deliverable energy density at high rate. The improved function of this designed interface relative to conventional electrode fabrication strategies is further highlighted.

25 ENERGY STORAGE↗
DOE OSTI2017

Understanding materials challenges for rechargeable ion batteries with in situ transmission electron microscopy

An in-depth understanding of material behaviours under complex electrochemical environment is critical for the development of advanced materials for the next-generation rechargeable ion batteries. The dynamic conditions inside a working battery had not been intensively explored until the advent of various in situ characterization techniques. Real-time transmission electron microscopy of electrochemical reactions is one of the most significant breakthroughs poised to enable radical shift in our knowledge on how materials behave in the electrochemical environment. This review, therefore, summarizes the scientific discoveries enabled by in situ transmission electron microscopy, and specifically emphasizes the applicability of this technique to address the critical challenges in the rechargeable ion battery electrodes, electrolyte and their interfaces. New electrochemical systems such as lithium–oxygen, lithium–sulfur and sodium ion batteries are included, considering the rapidly increasing application of in situ transmission electron microscopy in these areas. A systematic comparison between lithium ion-based electrochemistry and sodium ion-based electrochemistry is also given in terms of their thermodynamic and kinetic differences. The effect of the electron beam on the validity of in situ observation is also covered. This review concludes by providing a renewed perspective for the future directions of in situ transmission electron microscopy in rechargeable ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2022

Microbial biofilms as living photoconductors due to ultrafast electron transfer in cytochrome OmcS nanowires

Light-induced microbial electron transfer has potential for efficient production of value-added chemicals, biofuels and biodegradable materials owing to diversified metabolic pathways. However, most microbes lack photoactive proteins and require synthetic photosensitizers that suffer from photocorrosion, photodegradation, cytotoxicity, and generation of photoexcited radicals that are harmful to cells, thus severely limiting the catalytic performance. Therefore, there is a pressing need for biocompatible photoconductive materials for efficient electronic interface between microbes and electrodes. Here we show that living biofilms of Geobacter sulfurreducens use nanowires of cytochrome OmcS as intrinsic photoconductors. Photoconductive atomic force microscopy shows up to 100-fold increase in photocurrent in purified individual nanowires. Photocurrents respond rapidly (<100 ms) to the excitation and persist reversibly for hours. Femtosecond transient absorption spectroscopy and quantum dynamics simulations reveal ultrafast (~200 fs) electron transfer between nanowire hemes upon photoexcitation, enhancing carrier density and mobility. Our work reveals a new class of natural photoconductors for whole-cell catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

The role of alkali metal cations and platinum-surface hydroxyl in the alkaline hydrogen evolution reaction

The platinum-catalysed hydrogen evolution reaction (HER) generally shows poorer kinetics in alkaline electrolyte and represents a key challenge for alkaline water electrolysis. In the presence of alkali metal cations and hydroxyl anions, the electrode–electrolyte (platinum–water) interface in an alkaline electrolyte is far more complex than that in an acidic electrolyte. Here we combine electrochemical impedance spectroscopy and an electrical transport spectroscopy approach to probe and understand the fundamental role of different cations (Li + , Na + and K + ) in HER kinetics. Our integrated studies suggest that the alkali metal cations play an indirect role in modifying the HER kinetics, with the smaller cations being less destabilizing to the hydroxyl adsorbate (OH ad ) species in the HER potential window, which favours a higher coverage of OH ad on the platinum surface. Here, the surface OH ad species are highly polar and act as both electronically favoured proton acceptors and geometrically favoured proton donors to promote water dissociation in alkaline media, thus boosting the Volmer-step kinetics and the HER activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Sulfide glass solid-state electrolyte separators for Li metal batteries: using an interlayer to increase rate performance and reduce stack pressure

We report on the solubility of (Li 2 S) 60 (SiS 2 ) x (P 2 S 5 ) 40–x , (0 ≤ x ≤ 40) sulfide glass solid-state electrolytes in the 1:1 (v/v) DME:DOL solvent mixture, a popular choice for lithium metal battery liquid electrolytes. SiS 2 -rich glasses within the compositional range of (Li 2 S) 60 (SiS 2 ) x (P 2 S 5 ) 40–x (28 ≤ x ≤ 40) were found to be functionally insoluble in DME:DOL. Hybrid symmetric test cells with a thin liquid electrolyte layer (0.6 M LiTFSI + 0.4 M LiNO 3 in 1:1 (v/v) DME:DOL) at the interface between lithium metal electrodes and an insoluble (Li 2 S) 60 (SiS 2 ) 28 (P 2 S 5 ) 12 glass wafer were tested. Hybrid test cells delivered a critical current density of 3.0 mA cm –2 at 25 °C and 0.1 MPa, which is nearly double the CCD of comparable dry symmetric test cells cycled at 10× higher stack pressure.

25 ENERGY STORAGE↗
DOE OSTI2022

Observation of the surface layer of lithium metal using in situ spectroscopy

In this work, we have investigated the surface of lithium metal using x-ray photoemission spectroscopy and optical spectroscopic ellipsometry. Even if we prepare the surface of lithium metal rigorously by chemical cleaning and mechanical polishing inside a glovebox, both spectroscopic investigations show the existence of a few tens of nanometer-thick surface layers, consisting of lithium oxides and lithium carbonates. When lithium metal is exposed to room air (~50% moisture), in situ real-time monitoring of optical spectra indicates that the surface layer grows at a rate of approximately 24 nm/min, presumably driven by an interface-controlled process. Our results hint that surface-layer-free lithium metals are formidable to achieve by a simple cleaning/polishing method, suggesting that the initial interface between lithium metal electrodes and solid-state electrolytes in fabricated lithium metal batteries can differ from an ideal lithium/electrolyte contact.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Deriving effective electrode–ion interactions from free-energy profiles at electrochemical interfaces

Understanding ion adsorption at electrified metal–electrolyte interfaces is essential for accurate modeling of electrochemical systems. Here, in this study, we systematically investigate the free energy profiles of Na + , Cl − , and F − ions at the Au(111)–water interface using enhanced sampling molecular dynamics with both classical force fields and machine-learned interatomic potentials (MLIPs). Our classical metadynamics results reveal a strong dependence of predicted ion adsorption on the Lennard-Jones parameters, highlighting that—without due care—standard mixing rules can lead to qualitatively incorrect descriptions of ion–metal interactions. We present a systematic methodology for tuning the cross term LJ parameters to control adsorption energetics in agreement with more accurate models. As a surrogate for an ab initio model, we employed the recently released Universal Models for Atoms MLIP, which validates classical trends and displays strong specific adsorption for chloride, weak adsorption for fluoride, and no specific adsorption for sodium, in agreement with experimental and theoretical expectations. By integrating molecular-level adsorption free energies into continuum models of the electric double layer, we show that specific ion adsorption substantially alters the interfacial ion population, the potential of zero charge, and the differential capacitance of the system. Our results underscore the critical importance of force field parameterization and advanced interatomic potentials for the predictive modeling of ion-specific effects at electrified interfaces and provide a robust framework for bridging molecular simulations and continuum electrochemical models.

Roncoroni, Fabrice [Lawrence Berkeley National Lab↗
DOE OSTI2020

Gap states and valley-spin filtering in transition metal dichalcogenide monolayers

The magnetically induced valley-spin filtering in transition metal dichalcogenide monolayers ($\textit{MX}_2$, where $\textit{M}$ = Mo, W and X = S, Se, Te) promises a new paradigm in information processing. However, the detailed understanding of this effect is still limited, regarding its underlying transport processes. As such, herein it is suggested that the filtering mechanism can be greatly elucidated by the concept of metal-induced gap states (MIGS), appearing in the electrode-terminated $\textit{MX}_2$ materials, i.e., the referential filter setup. In particular, the gap states are predicted here to mediate valley- and spin-resolved charge transport near the ideal electrode/$\textit{MX}_2$ interface, and therefore to initiate filtering. It is also argued that the role of MIGS increases when the channel length is diminished, as they begin to govern the overall valley-spin transport in the tunneling regime. In what follows, the presented study yields fundamental scaling trends for the valley-spin selectivity with respect to the intrinsic physics of the filter materials. As a result, it facilitates insight into the analyzed effects and provides design guidelines toward efficient valley-spin filter devices that are based on the discussed materials or other hexagonal monolayers with a broken inversion symmetry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Imaging, understanding, and control of nanoscale materials transformations

The development of liquid cells for transmission electron microscopy has enabled breakthroughs in our ability to follow nanoscale structural, morphological, or chemical changes during materials growth and applications. Time-resolved high-resolution imaging and chemical analysis through liquids opened the opportunity to capture nanoscale dynamic processes of materials, including reaction intermediates and the transformation pathways. In this article, a series of work is highlighted with topics ranging from liquid cell developments to in situ studies of nanocrystal growth and transformations, dendrite formation, and suppression of lithium dendrites through in situ characterization of the solid–electrolyte interphase chemistry. The understanding garnered is expected to accelerate the discovery of novel materials for applications in energy storage, catalysis, sensors, and other functional devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Thermodynamic, Kinetic and Electrochemical Studies on Mixed Proton, Oxygen Ion and Electron (Hole) Conductors

The report contains a summary of work done during the period of performance September 1, 2015 through August 31, 2021. The principal objective of the work was to conduct thermodynamic, kinetic and electrochemical studies on mixed proton, oxygen ion and electron (hole) conductors. The project also involved studies on cation conductors such as Li + and Na + ion conductors of particular relevance to batteries. The work involved theory and experiments. Since any use of ionic conductors necessarily entails two electrodes, electrode reactions are central to the overall transport processes from one electrode, through the electrolyte, to the other electrode. The role of interfaces and electrochemical reactions is thus of central importance. Transport processes in fuel cells, electrolyzers, lithium batteries and sodium batteries were examined using linear non-equilibrium thermodynamics, which is based on the assumption of small departures from thermodynamic equilibrium. The main approach involved expressing transport processes using the Onsager equations which naturally include coupling of thermodynamic flows and thermodynamic forces. The basic tenet of linear nonequilibrium thermodynamics is the existence of local thermodynamic equilibrium which means that all thermodynamic functions are locally defined. Thus, chemical potentials of various species are defined locally as a function of position and also of time. The existence of local thermodynamic equilibrium has fundamental implications concerning transport of electronic species through a predominantly ionic conductor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Compatibility issues between electrodes and electrolytes in solid-state batteries

Remarkable success has been achieved in the discovery of ceramic alkali superionic conductors as electrolytes in solid-state batteries; however, obtaining a stable interface between these electrolytes and electrodes is difficult. Only limited studies on the compatibility between electrodes and solid electrolytes have been reported, partially because of the need for expensive instrumentation and special cell designs. Without simple yet powerful tools, these compatibility issues cannot be systematically investigated, thus hindering the generalization of design rules for the integration of solid-state battery components. Herein, we present a methodology that combines density functional theory calculations and simple experimental techniques such as X-ray diffraction, simultaneous differential scanning calorimetry and thermal gravimetric analysis, and electrochemistry to efficiently screen the compatibility of numerous electrode/electrolyte pairs. We systemically distinguish between the electrochemical stability of the solid-state conductor, which is relevant wherever the electrolyte contacts an electron pathway, and the electrochemical stability of the electrode/electrolyte interfaces. For the solid electrolyte, we are able to computationally derive an absolute thermodynamic stability voltage window, which is small for Na 3 PS 4 and Na 3 PSe 4 , and a larger voltage window which can be kinetically stabilized. The experimental stability, when measured with reliable techniques, falls between these thermodynamic and kinetic limits. Employing a Na solid-state system as an example, we demonstrate the efficiency of our method by finding the most stable system (NaCrO 2 |Na 3 PS 4 |Na–Sn) within a selected chemical space (more than 20 different combinations of electrodes and electrolytes). Important selection criteria for the cathode, electrolyte, and anode in solid-state batteries are also derived from this study. The current method not only provides an essential guide for integrating all-solid-state battery components but can also significantly accelerate the expansion of the electrolyte/electrode compatibility data.

25 ENERGY STORAGE↗
DOE OSTI2018

Suggestion of an Indicator to Evaluate Material Deposition in Resistance Spot Welding: Weld–Surface Interaction Index

Resistance spot welding (RSW) is still leading joining process in the automotive industry due to the simplicity and speed of the process. On the other hand, galvanized steel sheets provide improvement in corrosion resistance of the auto body. Material deposition has an influence on the corrosion resistance and weld strength; however, in the literature very little effort has been made to identify any weld–surface interaction numerically. In this study, a numerical approach called “Weld–Surface Interaction Index” (I{sub WSI}) has been introduced to investigate the effect of material deposition on the corrosion sensitivity of the welding zone and its periphery. A systematic investigation was carried out to better understand the effects of an electrode cap–galvanized steel sheet interface on the corrosion resistance of spot-welded steel. The chemical composition of DP600 steel sheet and Z-Trode electrode cap was analyzed by using a spectrometer. The specimens were then joined by using same caps up to 1200 welds. SEM–EDS analysis was also performed on the chosen specimens to determine the weight percentages (wt.%) of Fe, Zn and Cu. EDS analysis results and coefficient of variation wt.% of Fe, Zn and Cu were used to compose I{sub WSI} formula. In the proposed formula, wt.% of Zn represented resistivity of the cover to corrosion, while wt.% of Fe represents the vulnerability.

36 MATERIALS SCIENCE↗
NASA NTRS1999

Electric Field Induced Interfacial Instabilities

The study of the interface in a charge-free, critical and near-critical binary fluid in the presence of an externally applied electric field is presented. At sufficiently large fields, the interface between the two phases of the binary fluid should become unstable and exhibit an undulation with a predefined wavelength on the order of the capillary length. As the critical point is approached, this wavelength is reduced, potentially approaching length-scales such as the correlation length or critical nucleation radius. At this point the critical properties of the system may be affected. In this paper, the flat interface of a marginally polar binary fluid mixture is stressed by a perpendicular alternating electric field and the resulting instability is characterized by the critical electric field E(sub c) and the pattern observed. The character of the surface dynamics at the onset of instability is found to be strongly dependent on the frequency f of the field applied. The plot of E(sub c) vs. f for a fixed temperature shows a sigmoidal shape, whose low and high frequency limits are well described by a power-law relationship, E(sub c) = epsilon(exp zeta) with zeta = 0.35 and zeta = 0.08, respectively. The low-limit exponent compares well with the value zeta = 4 for a system of conducting and non-conducting fluids. On the other hand, the high-limit exponent coincides with what was first predicted by Onuki. The instability manifests itself as the conducting phase penetrates the non-conducting phase. As the frequency increases, the shape of the pattern changes from an array of bifurcating strings to an array of column-like (or rod-like) protrusions, each of which spans the space between the plane interface and one of the electrodes. For an extremely high frequency, the disturbance quickly grows into a parabolic cone pointing toward the upper plate. As a result, the interface itself changes its shape from that of a plane to that of a high sloping pyramid.

Kusner, Robert E.↗
NASA NTRS1992

Enhanced fatigue and retention in ferroelectric thin film memory capacitors by post-top electrode anneal treatment

Thin film ferroelectric capacitors comprising a ferroelectric film sandwiched between electrodes for nonvolatile memory operations are rendered more stable by subjecting the capacitors to an anneal following deposition of the top electrode. The anneal is done so as to form the interface between the ferroelectric film and the top electrode. Heating in an air oven, laser annealing, or electron bombardment may be used to form the interface. Heating in an air oven is done at a temperature at least equal to the crystallization temperature of the ferroelectric film. Where the ferroelectric film comprises lead zirconate titanate, annealing is done at about 550 to 600 C for about 10 to 15 minutes. The formation treatment reduces the magnitude of charge associated with the nonswitching pulse in the thin film ferroelectric capacitors. Reduction of this charge leads to significantly more stable nonvolatile memory operations in both digital and analog memory devices. The formation treatment also reduces the ratio of change of the charge associated with the nonswitching pulse as a function of retention time. These improved memory devices exhibit greater performance in retention and reduced fatigue in memory arrays.

Thakoor, Sarita↗